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single-atom catalysis enables long-life, high-energy lithium-sulfur batteries

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Nano Research 2020年第7期13卷 1856-1866页

作者： Zechao Zhuang Qi Kang Dingsheng Wang Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Polymer Science and Engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China

With high energy density and low material cost,lithium sulfur batteries(LSBs)emerge quite expeditiously as a fascinating energy storage system over the past decade.Broad applications of LSBs ranging from electric vehicles to stationary grid storage seem rather bright in recent literatures.However,there still exist many pressing challenges to be addressed because we do not yet fully understand and control the electrode-electrolyte interface chemistries during battery operation,such as polysulide shuttling and poor utilization of active sulfur.single-atom catalysts(SACs)pave new possibilities of tackling the tough issues due to their decent applicability in the atomic-level identification of structure-activity relationships and reaction mechanism,as well as their structural tunability with atomic precision.This review comprehensively summarizes the very recent advances in utilization of highly active SACs for LSBs by stating and discussing the related publications,which involves catalyst synthesis routes,battery pertormance,catalytic mechanisms,optimization strategies,and promises to achieve long-lite,high-energy LSBs.We see that endeavors to employ SACs to modify sulfur cathode have allowed efficient polysulfide conversion and confinement,leading to the minimization of shuttle effect.Parallel efforts are being devoted to extending the scope of SACs to cell separator and lithium metal anode in order to unlock the full potential of LSBs.We also obtain mechanistic insights into battery chemistries and nature of SACs in their strong interactions with polysulfides through advanced in situ characterizations documented.Overall,acceleration in the development of LSBs by introducing SACs is noticeable,and this cutting edge needs more attentions to further promoting the design of better LSBs.

关键词： single-atom catalysis lithium-sulfur battery polysulfide conversion shuttle effect atomic-level insight

single-atom catalysis: a new field that learns from tradition

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National Science Review 2018年第5期5卷 690-693页

作者： Philip Ball NSR

Much of industrial chemical processing (in the petrochemicals industry, for example), and a great deal of laboratory chemical synthesis,involves catalysts that both lower the energy barrier to reaction and may help steer a reaction along a particular path. Traditionally,catalysts have come in two classes:heterogeneous, typically meaning that the catalyst is an extended solid; and homogeneous, where the catalyst is a small molecule that shares a solvent with the reactants. In heterogeneous catalysis, the reaction generally takes place on a

关键词： single-atom catalysis

single-atom catalysis for organic reactions

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Chinese Chemical Letters 2023年第6期34卷 121-129页

作者： Hanyu Hu Jiangbo Xi Key Laboratory of Novel Biomass-Based Environmental and Energy Materials in Petroleum and Chemical Industry Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemistry and Environmental EngineeringWuhan Institute of TechnologyWuhan 430205China

Metal-based catalysis,including homogeneous and heterogeneous catalysis,plays a significant role in the modern chemical industry.Heterogeneous catalysis is widely used due to the high efficiency,easy catalyst separation and recycling.However,the metal-utilization efficiency for conventional heterogeneous catalysts needs further improvement compared to homogeneous catalyst.To tackle this,the pursing of heterogenizing homogeneous catalysts has always been attractive but challenging.As a recently emerging class of catalytic material,single-atom catalysts(SACs)are expected to bridge homogeneous and heterogeneous catalytic process in organic reactions and have arguably become the most active new frontier in catalysis field.In this review,a brief introduction and development history of single-atom catalysis and SACs involved organic reactions are documented.In addition,recent advances in SACs and their practical applications in organic reactions such as oxidation,reduction,addition,coupling reaction,and other organic reactions are thoroughly reviewed.To understand structure-property relationships of single-atom catalysis in organic reactions,active sites or coordination structure,metal atom-utilization efficiency(e.g.,turnover frequency,TOF calculated based on active metal)and catalytic performance(e.g.,conversion and selectivity)of SACs are comprehensively summarized.Furthermore,the application limitations,development trends,future challenges and perspective of SAC for organic reaction are discussed.

关键词： single-atom catalysis Active site Metal utilization Organic reaction Catalytic performance

single Cu atom dispersed on S,N-codoped nanocarbon derived from shrimp shells for highly-efficient oxygen reduction reaction

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Nano Research 2022年第7期15卷 5995-6000页

作者： Hao Zhang Qingdi Sun Qian He Ying Zhang Xiaohui He Tao Gan Hongbing Ji Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275China School of Chemistry and Chemical Engineering Guangxi UniversityNanning 530004China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China

Recently,Cu-based single-atom catalysts(SACs)have garnered increasing attention as substitutes for platinum-based catalysts in the oxygen reduction reaction(ORR).Therefore,a facile,economical,and efficient synthetic methodology for the preparation of a high-performance Cu-based SAC electrocatalyst for the ORR is extremely desired,but is also significantly challenging.In this study,we propose a ball-milling method to synthesize isolated metal SACs embedded in S,N-codoped nanocarbon(MNSDC,M=Cu,Fe,Co,Ni,Mn,Pt,and Pd).In particular,the Cu-NSDC SACs exhibit high electrochemical activity for the ORR with half-wave potential(E_(1/2))of 0.84 V(vs.reversible hydrogen electrode(RHE),20 mV higher than Pt/C)in alkaline electrolyte,excellent stability,and electrocatalytic selectivity.Density functional theory(DFT)calculations demonstrated that the desorption of OH*intermediates was the rate-determining step over Cu-NSDC.This study creates a pathway for high-performance ORR single atomic electrocatalysts for fuel cell applications and provides opportunities to convert biowaste materials into commercial opportunities.

关键词： ball milling oxygen reduction reaction single-atom catalysis shrimp shell S,N-codoped nanocarbon

single-atom cobalt nanozymes promote spinal cord injury recovery by anti-oxidation and neuroprotection

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Nano Research 2023年第7期16卷 9752-9759页

作者： Yuxing Jiang Hongtao Rong Yifan Wang Shange Liu Peng Xu Zhen Luo Lamei Guo Tao Zhu(✉) Hongpan Rong Dingsheng Wang Jiatao Zhang Yu Yi Hao Wang Tianjin Medical University General Hospital Tianjin 300052China CAS Center for Excellence in Nanoscience CAS Key Laboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and TechnologyBeijing 100190China Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Key Laboratory of Medical Molecule Science and Pharmaceutics EngineeringMinistry of Industry and Information TechnologySchool of Materials Science&EngineeringSchool of Chemistry and Chemical EngineeringInstitute of Engineering MedicineBeijing Institute of TechnologyBeijing 100081China Department of Chemistry Tsinghua UniversityBeijing 100084China University of Chinese Academy of Sciences Beijing 100049China

Oxidative stress and inflammation are central pathophysiological processes in a traumatic spinal cord injury(SCI).Antioxidant therapies that reduce the reactive oxygen and nitrogen species(RONS)overgeneration and inflammation are proved promising for improving the outcomes.However,efficient and long-lasting antioxidant therapy to eliminate multiple RONS with effective neuroprotection remains challenging.Here,a single-atom cobalt nanozyme(Co-SAzyme)with a hollow structure was reported to reduce the RONS and inflammation in the secondary injury of SCI.Among SAzymes featuring different single metal-N sites(e.g.,Mn,Fe,Co,Ni,and Cu),this Co-SAzyme showed a versatile property to eliminate hydrogen peroxide(H_(2)O_(2)),superoxide anion(O_(2)·^(-)),hydroxyl radical(·OH),nitric oxide(·NO),and peroxynitrite(ONOO^(-))that overexpressed in the early stage of SCI.The porous hollow structure also allowed the encapsulation and sustained release of minocycline for neuroprotection in synergy.In vitro results showed that the Co-SAzyme reduced the apoptosis and pro-inflammatory cytokine levels of microglial cells under oxidative stress.In addition,the Co-SAzyme combined with minocycline achieved remarkable improved functional recovery and neural repairs in the SCI-rat model.

关键词： single-atom catalysis spinal cord injury reactive oxygen and nitrogen species anti-inflammation neuroprotection

How water molecules occupying the active site of a single-atom catalyst affect the electrochemical reduction of carbon dioxide

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Nano Research 2023年第7期16卷 9091-9098页

作者： Jia Zhao Di Liu Fenfei Wei Weng Fai Ip Hui Pan Sen Lin State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350002China Institute of Applied Physics and Materials Engineering University of MacaoTaipa 999078MacaoChina Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoTaipa 999078MacaoChina

In single-atom catalysts(SACs),the single atoms are often exposed as protrusions above the substrate.The solvent molecules in the electrocatalytic environment can interact or even bind to these coordination-unsaturated single atoms and thus influence the reaction process,but this has not been studied in depth.In this work,we systematically investigate the thermodynamics of CO_(2)reduction reaction(CO_(2)RR)to CO over MoS_(2)-supported single metal atom catalysts(TM@MoS_(2),TM=transition metal)under vacuum and explicit solvent environments using density functional theory.In addition,the ab initio molecular dynamics results show that explicit H_(2)O molecules can coordinate to the TM site and undergo competitive adsorption with the CO_(2)RR intermediates,which significantly affects the energy and conformation of the CO_(2)RR pathway.Electronic structure analysis reveals that the occupying H_(2)O molecules change the electronic state of single atom and further influence the adsorption strength of different CO_(2)RR intermediates.Our work shows that water molecules can not only act as ligands to influence the electronic state of TM,but also affect the energy and conformation of CO_(2)RR intermediates,which highlights the important role of occupying H_(2)O molecules at the single-atom sites in CO_(2)RR and provides useful insights for the design of SACs for efficient CO_(2)RR.

关键词： electrocatalytic CO_(2)reduction solvent effect single-atom catalysis density functional theory ab initio molecular dynamics

Cu_(1)-B dual-active sites catalysts for the efficient dehydrogenative coupling and CO_(2)electroreduction

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Nano Research 2023年第4期16卷 4582-4588页

作者： Konglin Wu Zhaobin Fang Cheng Peng Yining Zhang Binbin Jiang Yanshang Kang Zhiming Chen Mingfu Ye Yuxi Wu Xianwen Wei Shoujie Liu Sha Li Jian Zhang Key Laboratory of Metallurgical Emission Reduction&Resources Recycling of Ministry of Education Anhui University of TechnologyMaanshan 243002China Anhui Laboratory of Clean Catalytic Engineering School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China Institute of Clean Energy and Advanced Nanocatalysis(iClean) School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515063China Institute of Molecular Plus Tianjin UniversityTianjin 300072China School of Chemistry and Chemical Engineering Anqing Normal UniversityAnqing 246001China Jiangxi Province Engineering Research Center of Ecological Chemical Industry Jiujiang UniversityJiujiang 332005China College of Chemistry and Materials Engineering Wenzhou UniversityWenzhou 325035China

Dual-active sites(DASs)catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects.Therefore,the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now.In this work,we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material(Cu_(1)-B/NPC).Numerous systematic characterization and density functional theoretical(DFT)calculation results showed that the Cu and B existed as Cu-N4 porphyrinlike unit and B-N_(3)unit in the obtained catalyst.DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu_(1)-B-N6 dual-sites.The Cu_(1)-B/NPC catalyst was more effective than the single-active site catalysts with B-N_(3)sites in NPC(B/NPC)and Cu-N4 porphyrin-like sites in NPC(Cu_(1)/NPC),respectively,for the dehydrogenative coupling of dimethylphenylsilane(DiMPSH)with various alcohols,performing the great activity(>99%)and selectivity(>99%).The catalytic performances of the Cu_(1)-B/NPC catalyst remained nearly unchanged after five cycles,also indicating its outstanding recyclability.DFT calculations showed that the Cu_(1)-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N_(3)and Cu-N4 porphyrin-like sites.Furthermore,the rate-limiting step of dehydrogenation of DiMPSH on Cu_(1)-B-N6 dual-sites also showed a much lower activation energy than the other two single sites.Benefitting from the superiority of the Cu_(1)-B-N6 dual-sites,the Cu_(1)-B/NPC catalyst can also be used for CO_(2)electroreduction to produce syngas.Thus,DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.

关键词： dual-active sites single-atom catalysis porous carbon dehydrogenative coupling

Construction of highly dispersed Pt single sites and high-efficiencyheterocatalysis silylation of alcohols with silanes

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Nano Research 2023年第4期16卷 4643-4649页

作者： Qiulian Wei Yunqiang Sun Shan Wang Zunfu Hu Qingyun Liu Xiuwen Zheng School of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266510China Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong College of Chemistry and Chemical EngineeringLinyi UniversityLinyi 276000China

The construction of silicon-oxygen bonds has been highlighted as an exciting achievement in organosilicon and green chemistry,but their synthetic efficiency has great improvement potential,so it is crucial to explore and achieve an effective approach for synthesizing such compounds.In this study,we successfully prepared the highly dispersed platinum single-atom catalyst(Pt SAC/N-C)through a coordination-assisted strategy with a mixture of ligands(H2bpdc and H2bpydc),which were used for the Osilylation of alcohols with silanes.The strong coordination between Pt2+and the Pyridine N at the skeleton of UiO-67 plays a critical role in accessing the atomically isolated dispersion of Pt sites.Without the assistance of the H2bpydc ligands,the Pt/UiO-67-bpdc precursor is prone to aggregation during the pyrolysis process,resulting in the formation of Pt nanoparticles.Aided by advanced characterization techniques of high-angle annular dark-field scanning transmission electron microscopy(HAADFSTEM)and X-ray absorption fine structure(XAFS)spectroscopy,it has been demonstrated that atomically dispersed Pt was formed on the UiO-67 through a local structure of four-coordinated Pt-N4,exhibiting a high actual Pt loading content(0.6962 wt.%).In the oxidation of silanes,the Pt SAC/N-C catalyst showed a high turnover frequency(TOF)value(up to 9,920 h−1)when the catalyst loading decreased to 0.005%.Excellent performance was maintained during recycling experiments,indicating high stability of the catalyst.

关键词： high-dispersion single-atom catalysis O-silylation heterogeneous catalysis

single-atom Cu anchored on N-doped graphene/carbon nitride heterojunction for enhanced photocatalytic H_(2)O_(2) production

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Journal of Materials Science & Technology 2023年第30期161卷 192-200页

作者： Han Li Bicheng Zhu Bei Cheng Guoqiang Luo Jingsan Xu Shaowen Cao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China School of Chemistry and Physics Queensland University of TechnologyBrisbaneQLD 4000Australia

Photocatalytic production of H_(2)O_(2) by polymeric carbon nitride has been regarded as a promising ap-proach for the conversion of solar energy into valuable chemicals.However,the efficiency of pristine car-bon nitride is limited by the rapid charge recombination and the lack of suitable active sites.Herein,we introduce single-atom Cu anchored on N-doped graphene(Cu-NG)as a cocatalyst coupled with carbon nitride via covalent bonding to enhance photocatalytic H_(2)O_(2) production.The Cu-NG/carbon nitride could broaden the light absorption from UV to near-infrared region,contributing to the photocatalytic process.Moreover,NG containing electron-rich N atoms could serve as anchoring sites for stabilizing single-atom Cu.Importantly,the single-atom Cu acts not only as an electron sink to steer the interfacial charge sep-aration but also as an active site for molecular oxygen adsorption and activation.With the synergistic effect of the enhanced interfacial charge separation and suitable active sites,Cu-NG/carbon nitride ex-hibits improved photocatalytic performance with an H_(2)O_(2) generation rate of 2856μmol g^(−1)h^(−1),which is 2.6 times that of pristine carbon nitride.This work provides a protocol for high-performance photocat-alytic H_(2)O_(2) production using a single-atom cocatalyst.

关键词： single-atom catalysis Interfacial charge separation Photocatalytic H_(2)O_(2)production